Printable enzyme-embedded materials for methane to methanol conversion

Blanchette, Craig D.; Knipe, Jennifer M.; Stolaroff, Joshuah K.; DeOtte, Joshua R.; Oakdale, James S.; Maiti, Amitesh; Lenhardt, Jeremy M.; Sirajuddin, Sarah; Rosenzweig, Amy C.; Baker, Sarah E.

doi:10.1038/ncomms11900

Title: Printable enzyme-embedded materials for methane to methanol conversion

Abstract

An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas. The only selective catalysts for methane activation and conversion to methanol under mild conditions are methane monooxygenases (MMOs) found in methanotrophic bacteria; however, these enzymes are not amenable to standard enzyme immobilization approaches. Using particulate methane monooxygenase (pMMO), we create a biocatalytic polymer material that converts methane to methanol. We demonstrate embedding the material within a silicone lattice to create mechanically robust, gas-permeable membranes, and direct printing of micron-scale structures with controlled geometry. Remarkably, the enzymes retain up to 100% activity in the polymer construct. The printed enzyme-embedded polymer motif is highly flexible for future development and should be useful in a wide range of applications, especially those involving gas–liquid reactions.

Authors:

Blanchette, Craig D. ^[1]; Knipe, Jennifer M. ^[1]; Stolaroff, Joshuah K. ^[1]; DeOtte, Joshua R. ^[1]; Oakdale, James S. ^[1]; Maiti, Amitesh ^[1]; Lenhardt, Jeremy M. ^[1]; Sirajuddin, Sarah ^[2]; Rosenzweig, Amy C. ^[2]; Baker, Sarah E. ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Northwestern Univ., Evanston, IL (United States)

Publication Date:: Wed Jun 15 00:00:00 EDT 2016

Research Org.:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1349013

Report Number(s):: LLNL-JRNL-678269
Journal ID: ISSN 2041-1723

Grant/Contract Number:: AC52-07NA27344

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 7; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 03 NATURAL GAS; 59 BASIC BIOLOGICAL SCIENCES

Citation Formats


                    Blanchette, Craig D., Knipe, Jennifer M., Stolaroff, Joshuah K., DeOtte, Joshua R., Oakdale, James S., Maiti, Amitesh, Lenhardt, Jeremy M., Sirajuddin, Sarah, Rosenzweig, Amy C., and Baker, Sarah E. Printable enzyme-embedded materials for methane to methanol conversion.  United States: N. p., 2016. 
Web.  doi:10.1038/ncomms11900.

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                    Blanchette, Craig D., Knipe, Jennifer M., Stolaroff, Joshuah K., DeOtte, Joshua R., Oakdale, James S., Maiti, Amitesh, Lenhardt, Jeremy M., Sirajuddin, Sarah, Rosenzweig, Amy C., & Baker, Sarah E. Printable enzyme-embedded materials for methane to methanol conversion.  United States.  https://doi.org/10.1038/ncomms11900

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                    Blanchette, Craig D., Knipe, Jennifer M., Stolaroff, Joshuah K., DeOtte, Joshua R., Oakdale, James S., Maiti, Amitesh, Lenhardt, Jeremy M., Sirajuddin, Sarah, Rosenzweig, Amy C., and Baker, Sarah E. Wed .  
"Printable enzyme-embedded materials for methane to methanol conversion".  United States.  https://doi.org/10.1038/ncomms11900.  https://www.osti.gov/servlets/purl/1349013.

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@article{osti_1349013,

  title        = {Printable enzyme-embedded materials for methane to methanol conversion},

  author       = {Blanchette, Craig D. and Knipe, Jennifer M. and Stolaroff, Joshuah K. and DeOtte, Joshua R. and Oakdale, James S. and Maiti, Amitesh and Lenhardt, Jeremy M. and Sirajuddin, Sarah and Rosenzweig, Amy C. and Baker, Sarah E.},

  abstractNote = {An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas. The only selective catalysts for methane activation and conversion to methanol under mild conditions are methane monooxygenases (MMOs) found in methanotrophic bacteria; however, these enzymes are not amenable to standard enzyme immobilization approaches. Using particulate methane monooxygenase (pMMO), we create a biocatalytic polymer material that converts methane to methanol. We demonstrate embedding the material within a silicone lattice to create mechanically robust, gas-permeable membranes, and direct printing of micron-scale structures with controlled geometry. Remarkably, the enzymes retain up to 100% activity in the polymer construct. The printed enzyme-embedded polymer motif is highly flexible for future development and should be useful in a wide range of applications, especially those involving gas–liquid reactions.},

  doi          = {10.1038/ncomms11900},

  journal      = {Nature Communications},

  number       = ,

  volume       = 7,

  place        = {United States},

  year         = {Wed Jun 15 00:00:00 EDT 2016},

  month        = {Wed Jun 15 00:00:00 EDT 2016}

}

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DOI: 10.1039/c8ta07716a

Microfluidic immobilized enzyme reactors for continuous biocatalysis
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Zhu, Yujiao; Chen, Qingming; Shao, Liyang
Reaction Chemistry & Engineering, Vol. 5, Issue 1
DOI: 10.1039/c9re00217k

From micelles to bicelles: Effect of the membrane on particulate methane monooxygenase activity
journal, May 2018

Ro, Soo Y.; Ross, Matthew O.; Deng, Yue Wen
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Industrial biomanufacturing: The future of chemical production
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Science, Vol. 355, Issue 6320
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Particulate methane monooxygenase contains only mononuclear copper centers
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Ross, Matthew O.; MacMillan, Fraser; Wang, Jingzhou
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Industrial Applications of Enzymes: Recent Advances, Techniques, and Outlooks
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Chapman, Jordan; Ismail, Ahmed; Dinu, Cerasela
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Functionalized DNA-spider silk nanohydrogels for controlled protein binding and release
journal, March 2020

Humenik, Martin; Preiß, Tamara; Gödrich, Sebastian
Materials Today Bio, Vol. 6
DOI: 10.1016/j.mtbio.2020.100045

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Similar Records

Title: Printable enzyme-embedded materials for methane to methanol conversion

Abstract

Citation Formats

Catalysis Research of Relevance to Carbon Management: Progress, Challenges, and Opportunities journal, April 2001

Methanotrophs and copper journal, July 2010

Progress in enzymatic membrane reactors – a review journal, October 2004

Maleimide Cross-Linked Bioactive PEG Hydrogel Exhibits Improved Reaction Kinetics and Cross-Linking for Cell Encapsulation and In Situ Delivery journal, December 2011

Enrichment, Isolation and Some Properties of Methane-utilizing Bacteria journal, May 1970

Painting and Printing Living Bacteria: Engineering Nanoporous Biocatalytic Coatings to Preserve Microbial Viability and Intensify Reactivity journal, February 2007

Bioconversion of natural gas to liquid fuel: Opportunities and challenges journal, May 2014

Cross-linked redox gels containing glucose oxidase for amperometric biosensor applications journal, February 1990

Solubilisation of methane monooxygenase from Methylococcus capsulatus (Bath) journal, July 1989

Entrapment of Methyl Parathion Hydrolase in Cross-Linked Poly(γ-glutamic acid)/Gelatin Hydrogel journal, January 2014

Gas permeation through water-swollen hydrogel membranes journal, March 2008

Efficient immobilization of epoxide hydrolase onto silica gel and use in the enantioselective hydrolysis of racemic para-nitrostyrene oxide journal, March 2005

Immobilisation behaviour of biomolecules in mesoporous silica materials journal, September 2005

Preparation of water-swollen hydrogel membranes for gas separation journal, January 2001

Natural strategies for the spatial optimization of metabolism in synthetic biology journal, May 2012

Enzymatic Oxidation of Methane journal, March 2015

Engineering the third wave of biocatalysis journal, May 2012

The Leeuwenhoek Lecture 2000 The natural and unnatural history of methane-oxidizing bacteria journal, June 2005

Biocatalytic plastics as active and stable materials for biotransformations journal, August 1997

Substrate channeling and enzyme complexes for biotechnological applications journal, November 2011

Enabling Industrial Biocatalytic Processes by Application of Silicone-Coated Enzyme Preparations journal, September 2011

Pure and mixed gas CH4 and n-C4H10 permeability and diffusivity in poly(dimethylsiloxane) journal, December 2007

Oxidation of methane by a biological dicopper centre journal, April 2010

Gas Permeation and Diffusion in Cross-Linked Poly(ethylene glycol diacrylate) journal, May 2006

Three-Dimensional Printing of Elastomeric, Cellular Architectures with Negative Stiffness journal, May 2014

Photoinitiated Polymerization: Advances, Challenges, and Opportunities journal, August 2010

Bacteriohemerythrin bolsters the activity of the particulate methane monooxygenase (pMMO) in Methylococcus capsulatus (Bath) journal, June 2012

Blood Clot Initiation by Mesocellular Foams: Dependence on Nanopore Size and Enzyme Immobilization journal, December 2008

Hydrogels as Extracellular Matrices for Skeletal Tissue Engineering: State-of-the-Art and Novel Application in Organ Printing journal, August 2007

Gas and Vapor Solubility in Cross-Linked Poly(ethylene Glycol Diacrylate) journal, October 2005

Immobilization of Active Hydrogenases by Encapsulation in Polymeric Porous Gels journal, October 2005

Toward Delineating the Structure and Function of the Particulate Methane Monooxygenase from Methanotrophic Bacteria † journal, April 2004

Rethinking biological activation of methane and conversion to liquid fuels journal, April 2014

Ultralight, ultrastiff mechanical metamaterials journal, June 2014

Evidence for Oxygen Binding at the Active Site of Particulate Methane Monooxygenase journal, April 2012

The Effect of Cross-Linking on Gas Permeability in Cross-Linked Poly(Ethylene Glycol Diacrylate) journal, October 2005

Direct Catalytic Conversion of Methane to Methanol in an Aqueous Medium by using Copper-Promoted Fe-ZSM-5 journal, April 2012

The Membrane-Associated Methane Monooxygenase (pMMO) and pMMO-NADH:Quinone Oxidoreductase Complex from Methylococcus capsulatus Bath journal, September 2003

Purified particulate methane monooxygenase from Methylococcus capsulatus (Bath) is a dimer with both mononuclear copper and a copper-containing cluster journal, March 2003

Performance of Chloroperoxidase Stabilization in Mesoporous Sol-Gel Glass Using <I>In Situ</I> Glucose Oxidase Peroxide Generation journal, January 2004

Free radical-mediated oxidation of free amino acids and amino acid residues in proteins journal, July 2003

Structural Characteristics and Swelling Behavior of Poly(ethylene glycol) Diacrylate Hydrogels † journal, January 1996

Reaction mechanisms in the radiolysis of peptides, polypeptides, and proteins journal, April 1987

Enzymatic biofuel cells utilizing a biomimetic cofactor journal, January 2012

Perspective of Recent Progress in Immobilization of Enzymes journal, July 2011

Complete Oxidation of Methanol in Biobattery Devices Using a Hydrogel Created from Three Modified Dehydrogenases journal, December 2012

The solubility of hydrocarbon gases in lipid bilayers journal, November 1977

Cellular Solids: Three-Dimensional Printing of Elastomeric, Cellular Architectures with Negative Stiffness (Adv. Funct. Mater. 31/2014) journal, August 2014

Maleimide Cross-Linked Bioactive PEG Hydrogel Exhibits Improved Reaction Kinetics and Cross-Linking for Cell Encapsulation and In Situ Delivery journal, December 2011

Free radical-mediated oxidation of free amino acids and amino acid residues in proteins journal, July 2003

Bioconversion of natural gas to liquid fuel: Opportunities and challenges journal, May 2014

Immobilisation behaviour of biomolecules in mesoporous silica materials journal, September 2005

Bacteriohemerythrin bolsters the activity of the particulate methane monooxygenase (pMMO) in Methylococcus capsulatus (Bath) journal, June 2012

Release of protein from highly cross-linked hydrogels of poly(ethylene glycol) diacrylate fabricated by UV polymerization journal, May 2001

Characterization of permeability and network structure of interfacially photopolymerized poly(ethylene glycol) diacrylate hydrogels journal, July 1998

Organ printing: computer-aided jet-based 3D tissue engineering journal, April 2003

Cross-linked redox gels containing glucose oxidase for amperometric biosensor applications journal, February 1990

Enzymatic Oxidation of Methane journal, March 2015

Toward Delineating the Structure and Function of the Particulate Methane Monooxygenase from Methanotrophic Bacteria † journal, April 2004

Blood Clot Initiation by Mesocellular Foams: Dependence on Nanopore Size and Enzyme Immobilization journal, December 2008

Immobilization of Active Hydrogenases by Encapsulation in Polymeric Porous Gels journal, October 2005

Oxidation of methane by a biological dicopper centre journal, April 2010

Engineering the third wave of biocatalysis journal, May 2012

Biocatalytic plastics as active and stable materials for biotransformations journal, August 1997

Rethinking biological activation of methane and conversion to liquid fuels journal, April 2014

Purified particulate methane monooxygenase from Methylococcus capsulatus (Bath) is a dimer with both mononuclear copper and a copper-containing cluster journal, March 2003

Effects of Zinc on Particulate Methane Monooxygenase Activity and Structure journal, June 2014

Hydrogels as Extracellular Matrices for Skeletal Tissue Engineering: State-of-the-Art and Novel Application in Organ Printing journal, August 2007

Enrichment, Isolation and Some Properties of Methane-utilizing Bacteria journal, May 1970

Solubilisation of methane monooxygenase from Methylococcus capsulatus (Bath) journal, July 1989

Methanotrophs and copper journal, July 2010

Ultralight, ultrastiff mechanical metamaterials journal, June 2014

Production of High-Quality Particulate Methane Monooxygenase in High Yields from Methylococcus capsulatus (Bath) with a Hollow-Fiber Membrane Bioreactor journal, October 2003

Herstellung direkt nutzbarer Durchflussreaktorkartuschen durch 3D-Druck von thermostabilen Enzymen journal, April 2018

Metal–Organic Frameworks with Target‐Specific Active Sites Switched by Photoresponsive Motifs: Efficient Adsorbents for Tailorable CO 2 Capture journal, February 2019

On-Demand Production of Flow-Reactor Cartridges by 3D Printing of Thermostable Enzymes journal, April 2018

Metal–Organic Frameworks with Target‐Specific Active Sites Switched by Photoresponsive Motifs: Efficient Adsorbents for Tailorable CO 2 Capture journal, May 2019

Catalysis Research of Relevance to Carbon Management: Progress, Challenges, and Opportunities
journal, April 2001

Methanotrophs and copper
journal, July 2010

Progress in enzymatic membrane reactors – a review
journal, October 2004

Maleimide Cross-Linked Bioactive PEG Hydrogel Exhibits Improved Reaction Kinetics and Cross-Linking for Cell Encapsulation and In Situ Delivery
journal, December 2011

Enrichment, Isolation and Some Properties of Methane-utilizing Bacteria
journal, May 1970

Painting and Printing Living Bacteria: Engineering Nanoporous Biocatalytic Coatings to Preserve Microbial Viability and Intensify Reactivity
journal, February 2007

Bioconversion of natural gas to liquid fuel: Opportunities and challenges
journal, May 2014

Cross-linked redox gels containing glucose oxidase for amperometric biosensor applications
journal, February 1990

Solubilisation of methane monooxygenase from Methylococcus capsulatus (Bath)
journal, July 1989

Entrapment of Methyl Parathion Hydrolase in Cross-Linked Poly(γ-glutamic acid)/Gelatin Hydrogel
journal, January 2014

Gas permeation through water-swollen hydrogel membranes
journal, March 2008

Efficient immobilization of epoxide hydrolase onto silica gel and use in the enantioselective hydrolysis of racemic para-nitrostyrene oxide
journal, March 2005

Immobilisation behaviour of biomolecules in mesoporous silica materials
journal, September 2005

Preparation of water-swollen hydrogel membranes for gas separation
journal, January 2001

Natural strategies for the spatial optimization of metabolism in synthetic biology
journal, May 2012

Enzymatic Oxidation of Methane
journal, March 2015

Engineering the third wave of biocatalysis
journal, May 2012

The Leeuwenhoek Lecture 2000 The natural and unnatural history of methane-oxidizing bacteria
journal, June 2005

Biocatalytic plastics as active and stable materials for biotransformations
journal, August 1997

Substrate channeling and enzyme complexes for biotechnological applications
journal, November 2011

Enabling Industrial Biocatalytic Processes by Application of Silicone-Coated Enzyme Preparations
journal, September 2011

Pure and mixed gas CH4 and n-C4H10 permeability and diffusivity in poly(dimethylsiloxane)
journal, December 2007

Oxidation of methane by a biological dicopper centre
journal, April 2010

Gas Permeation and Diffusion in Cross-Linked Poly(ethylene glycol diacrylate)
journal, May 2006

Three-Dimensional Printing of Elastomeric, Cellular Architectures with Negative Stiffness
journal, May 2014

Photoinitiated Polymerization: Advances, Challenges, and Opportunities
journal, August 2010

Bacteriohemerythrin bolsters the activity of the particulate methane monooxygenase (pMMO) in Methylococcus capsulatus (Bath)
journal, June 2012

Blood Clot Initiation by Mesocellular Foams: Dependence on Nanopore Size and Enzyme Immobilization
journal, December 2008

Hydrogels as Extracellular Matrices for Skeletal Tissue Engineering: State-of-the-Art and Novel Application in Organ Printing
journal, August 2007

Gas and Vapor Solubility in Cross-Linked Poly(ethylene Glycol Diacrylate)
journal, October 2005

Immobilization of Active Hydrogenases by Encapsulation in Polymeric Porous Gels
journal, October 2005

Toward Delineating the Structure and Function of the Particulate Methane Monooxygenase from Methanotrophic Bacteria ^†
journal, April 2004

Rethinking biological activation of methane and conversion to liquid fuels
journal, April 2014

Ultralight, ultrastiff mechanical metamaterials
journal, June 2014

Evidence for Oxygen Binding at the Active Site of Particulate Methane Monooxygenase
journal, April 2012

The Effect of Cross-Linking on Gas Permeability in Cross-Linked Poly(Ethylene Glycol Diacrylate)
journal, October 2005

Direct Catalytic Conversion of Methane to Methanol in an Aqueous Medium by using Copper-Promoted Fe-ZSM-5
journal, April 2012

The Membrane-Associated Methane Monooxygenase (pMMO) and pMMO-NADH:Quinone Oxidoreductase Complex from Methylococcus capsulatus Bath
journal, September 2003

Purified particulate methane monooxygenase from Methylococcus capsulatus (Bath) is a dimer with both mononuclear copper and a copper-containing cluster
journal, March 2003

Performance of Chloroperoxidase Stabilization in Mesoporous Sol-Gel Glass Using <I>In Situ</I> Glucose Oxidase Peroxide Generation
journal, January 2004

Free radical-mediated oxidation of free amino acids and amino acid residues in proteins
journal, July 2003

Structural Characteristics and Swelling Behavior of Poly(ethylene glycol) Diacrylate Hydrogels ^†
journal, January 1996

Reaction mechanisms in the radiolysis of peptides, polypeptides, and proteins
journal, April 1987

Enzymatic biofuel cells utilizing a biomimetic cofactor
journal, January 2012

Perspective of Recent Progress in Immobilization of Enzymes
journal, July 2011

Complete Oxidation of Methanol in Biobattery Devices Using a Hydrogel Created from Three Modified Dehydrogenases
journal, December 2012

The solubility of hydrocarbon gases in lipid bilayers
journal, November 1977

Cellular Solids: Three-Dimensional Printing of Elastomeric, Cellular Architectures with Negative Stiffness (Adv. Funct. Mater. 31/2014)
journal, August 2014

Maleimide Cross-Linked Bioactive PEG Hydrogel Exhibits Improved Reaction Kinetics and Cross-Linking for Cell Encapsulation and In Situ Delivery
journal, December 2011

Free radical-mediated oxidation of free amino acids and amino acid residues in proteins
journal, July 2003

Bioconversion of natural gas to liquid fuel: Opportunities and challenges
journal, May 2014

Immobilisation behaviour of biomolecules in mesoporous silica materials
journal, September 2005

Bacteriohemerythrin bolsters the activity of the particulate methane monooxygenase (pMMO) in Methylococcus capsulatus (Bath)
journal, June 2012

Release of protein from highly cross-linked hydrogels of poly(ethylene glycol) diacrylate fabricated by UV polymerization
journal, May 2001

Characterization of permeability and network structure of interfacially photopolymerized poly(ethylene glycol) diacrylate hydrogels
journal, July 1998

Organ printing: computer-aided jet-based 3D tissue engineering
journal, April 2003

Cross-linked redox gels containing glucose oxidase for amperometric biosensor applications
journal, February 1990

Enzymatic Oxidation of Methane
journal, March 2015

Toward Delineating the Structure and Function of the Particulate Methane Monooxygenase from Methanotrophic Bacteria ^†
journal, April 2004

Blood Clot Initiation by Mesocellular Foams: Dependence on Nanopore Size and Enzyme Immobilization
journal, December 2008

Immobilization of Active Hydrogenases by Encapsulation in Polymeric Porous Gels
journal, October 2005

Oxidation of methane by a biological dicopper centre
journal, April 2010

Engineering the third wave of biocatalysis
journal, May 2012

Biocatalytic plastics as active and stable materials for biotransformations
journal, August 1997

Rethinking biological activation of methane and conversion to liquid fuels
journal, April 2014

Purified particulate methane monooxygenase from Methylococcus capsulatus (Bath) is a dimer with both mononuclear copper and a copper-containing cluster
journal, March 2003

Effects of Zinc on Particulate Methane Monooxygenase Activity and Structure
journal, June 2014

Hydrogels as Extracellular Matrices for Skeletal Tissue Engineering: State-of-the-Art and Novel Application in Organ Printing
journal, August 2007

Enrichment, Isolation and Some Properties of Methane-utilizing Bacteria
journal, May 1970

Solubilisation of methane monooxygenase from Methylococcus capsulatus (Bath)
journal, July 1989

Methanotrophs and copper
journal, July 2010

Ultralight, ultrastiff mechanical metamaterials
journal, June 2014

Production of High-Quality Particulate Methane Monooxygenase in High Yields from Methylococcus capsulatus (Bath) with a Hollow-Fiber Membrane Bioreactor
journal, October 2003

Herstellung direkt nutzbarer Durchflussreaktorkartuschen durch 3D-Druck von thermostabilen Enzymen
journal, April 2018

Metal–Organic Frameworks with Target‐Specific Active Sites Switched by Photoresponsive Motifs: Efficient Adsorbents for Tailorable CO ₂ Capture
journal, February 2019

On-Demand Production of Flow-Reactor Cartridges by 3D Printing of Thermostable Enzymes
journal, April 2018

Metal–Organic Frameworks with Target‐Specific Active Sites Switched by Photoresponsive Motifs: Efficient Adsorbents for Tailorable CO ₂ Capture
journal, May 2019

Techno-economic comparison of biogas cleaning for grid injection, compressed natural gas, and biogas-to-methanol conversion technologies: Techno-economic analysis of existing and emerging biogas upgrading technologies.
journal, February 2018

Improvement of bacterial methane elimination using porous ceramsite as biocarrier: Methane elimination using ceramsite as biocarrier
journal, March 2018

An efficient protein immobilization strategy: protein encapsulated in nano molecular cages
journal, April 2019